Rapid aerosol particle growth and increase of cloud condensation nucleus activity by secondary aerosol formation and condensation: A case study for regional air pollution in northeastern China
27 Jan 2009-Journal of Geophysical Research (John Wiley & Sons, Ltd)-Vol. 114, pp 1-13
TL;DR: In this article, a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN) was investigated.
Abstract:  This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1-month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (~30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m -3 h -1 during the late hours of the day. This growth rate was observed several times during the 1-month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07-0.86%, the CCN number concentrations reached maximum values of 4000-19,000 cm -3 only 6-14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1-0.3 to 0.35-0.5 for particles with diameters of 40-90 nm, but it remained nearly constant at ~0.45 for particles with diameters of ~190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.
TL;DR: A periodic cycle of PM episodes in Beijing is demonstrated that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles.
Abstract: As the world’s second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.
TL;DR: In this paper, the authors reviewed evidence of how climate change has already resulted in clearly discernable changes in marine Arctic ecosystems and found a total of 51 reports of documented changes in Arctic marine biota in response to climate change.
Abstract: In this article, we review evidence of how climate change has already resulted in clearly discernable changes in marine Arctic ecosystems. After defining the term ‘footprint’ and evaluating the availability of reliable baseline information we review the published literature to synthesize the footprints of climate change impacts in marine Arctic ecosystems reported as of mid-2009. We found a total of 51 reports of documented changes in Arctic marine biota in response to climate change. Among the responses evaluated were range shifts and changes in abundance, growth/condition, behaviour/phenology and community/regime shifts. Most reports concerned marine mammals, particularly polar bears, and fish. The number of well-documented changes in planktonic and benthic systems was surprisingly low. Evident losses of endemic species in the Arctic Ocean, and in ice algae production and associated community remained difficult to evaluate due to the lack of quantitative reports of its abundance and distribution. Very few footprints of climate change were reported in the literature from regions such as the wide Siberian shelf and the central Arctic Ocean due to the limited research effort made in these ecosystems. Despite the alarming nature of warming and its strong potential effects in the Arctic Ocean the research effort evaluating the impacts of climate change in this region is rather limited.
Beijing Normal University1, University of Maryland, College Park2, University of California, San Diego3, Chinese Academy of Sciences4, China Meteorological Administration5, Pacific Northwest National Laboratory6, Hebrew University of Jerusalem7, Princeton University8, California Institute of Technology9, Lanzhou University10, Nanjing University of Information Science and Technology11, University of Hawaii12, Kyushu University13, National Institute for Environmental Studies14, Vikram Sarabhai Space Centre15, Max Planck Society16
TL;DR: A comprehensive review of studies on Asian aerosols, monsoons, and their interactions is provided in this article, where a new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosolmonsoon climate system, subject to external forcing of global warming, anthropogenic aerosol, and land use and change.
Abstract: The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcing of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.
TL;DR: The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate.
Abstract: Organic substances can adopt an amorphous solid or semisolid state, influencing the rate of heterogeneous reactions and multiphase processes in atmospheric aerosols. Here we demonstrate how molecular diffusion in the condensed phase affects the gas uptake and chemical transformation of semisolid organic particles. Flow tube experiments show that the ozone uptake and oxidative aging of amorphous protein is kinetically limited by bulk diffusion. The reactive gas uptake exhibits a pronounced increase with relative humidity, which can be explained by a decrease of viscosity and increase of diffusivity due to hygroscopic water uptake transforming the amorphous organic matrix from a glassy to a semisolid state (moisture-induced phase transition). The reaction rate depends on the condensed phase diffusion coefficients of both the oxidant and the organic reactant molecules, which can be described by a kinetic multilayer flux model but not by the traditional resistor model approach of multiphase chemistry. The chemical lifetime of reactive compounds in atmospheric particles can increase from seconds to days as the rate of diffusion in semisolid phases can decrease by multiple orders of magnitude in response to low temperature or low relative humidity. The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate.
TL;DR: In this article, the authors review the major advances in aerosol measurements, PBL processes and their interactions with each other through complex feedback mechanisms, and highlight the priorities for future studies.
Abstract: Air quality is concerned with pollutants in both the gas phase and solid or liquid phases. The latter are referred to as aerosols, which are multifaceted agents affecting air quality, weather and climate through many mechanisms. Unlike gas pollutants, aerosols interact strongly with meteorological variables with the strongest interactions taking place in the planetary boundary layer (PBL). The PBL hosting the bulk of aerosols in the lower atmosphere is affected by aerosol radiative effects. Both aerosol scattering and absorption reduce the amount of solar radiation reaching the ground and thus reduce the sensible heat fluxes that drive the diurnal evolution of the PBL. Moreover, aerosols can increase atmospheric stability by inducing a temperature inversion as a result of both scattering and absorption of solar radiation, which suppresses dispersion of pollutants and leads to further increases in aerosol concentration in the lower PBL. Such positive feedback is especially strong during severe pollution events. Knowledge of the PBL is thus crucial for understanding the interactions between air pollution and meteorology. A key question is how the diurnal evolution of the PBL interacts with aerosols, especially in vertical directions, and affects air quality. We review the major advances in aerosol measurements, PBL processes and their interactions with each other through complex feedback mechanisms, and highlight the priorities for future studies.
TL;DR: In this paper, a method to describe the relationship between particle dry diameter and cloud condensation activity using a single hygroscopicity parameter is presented. But this method is limited to single and multi-component particles with varying amounts of inorganic, organic and surface active compounds.
Abstract: We present a method to describe the relationship between particle dry diameter and cloud condensation nu- clei (CCN) activity using a single hygroscopicity parameter . Values of the hygroscopicity parameter are between 0.5 and 1.4 for highly-CCN-active salts such as sodium chlo- ride, between 0.01 and 0.5 for slightly to very hygroscopic organic species, and 0 for nonhygroscopic components. Ob- servations indicate that atmospheric particulate matter is typ- ically characterized by 0.1<< 0.9. If compositional data are available and if the hygroscopicity parameter of each com- ponent is known, a multicomponent hygroscopicity parame- ter can be computed by weighting component hygroscopic- ity parameters by their volume fractions in the mixture. In the absence of information on chemical composition, exper- imental data for complex, multicomponent particles can be fitted to obtain the hygroscopicity parameter. The hygroscop- icity parameter can thus also be used to conveniently model the CCN activity of atmospheric particles, including those containing insoluble components. We confirm the applica- bility of the hygroscopicity parameter and its mixing rule by applying it to published hygroscopic diameter growth fac- tor and CCN-activation data for single- and multi-component particles containing varying amounts of inorganic, organic and surface active compounds. We suggest that may be fit to CCN data assuming s/a=0.072 J m 2 and present a table of derived for this value and T=298.15 K. The predicted hygroscopicities for mixtures that contain the surfactant ful- vic acid agree within uncertainties with the measured values. It thus appears that this approach is adequate for predict- ing CCN activity of mixed particles containing surface ac- tive materials, but the generality of this assumption requires further verification.
TL;DR: A global climate model used to investigate possible aerosol contributions to trends in China and India found precipitation and temperature changes in the model that were comparable to those observed if the aerosols included a large proportion of absorbing black carbon (“soot”), similar to observed amounts.
Abstract: In recent decades, there has been a tendency toward increased summer floods in south China, increased drought in north China, and moderate cooling in China and India while most of the world has been warming. We used a global climate model to investigate possible aerosol contributions to these trends. We found precipitation and temperature changes in the model that were comparable to those observed if the aerosols included a large proportion of absorbing black carbon ("soot"), similar to observed amounts. Absorbing aerosols heat the air, alter regional atmospheric stability and vertical motions, and affect the large-scale circulation and hydrologic cycle with significant regional climate effects.
TL;DR: The authors revisited common assumptions for estimating PM2.5 mass concentration and found that these assumptions can be used to estimate organic mass in a wide range of scenarios, such as PM1.5.
Abstract: (2001). Species Contributions to PM2.5 Mass Concentrations: Revisiting Common Assumptions for Estimating Organic Mass. Aerosol Science and Technology: Vol. 35, No. 1, pp. 602-610.
TL;DR: In this article, the authors describe an aerosol mass spectrometer (AMS) which has been developed in response to these aerosol sampling needs and demonstrate quantitative mea surement capability for a laboratory-generated pure component NH4 NO3 aerosol.
Abstract: The importance of atmospheric aerosols in regulating the Earth's climate and their potential detrimental impact on air quality and human health has stimulated the need for instrumentation which can provide real-time analysis of size resolved aerosol, mass, and chemical composition We describe here an aerosol mass spectrometer (AMS) which has been developed in response to these aerosol sampling needs and present results which demonstrate quantitative mea surement capability for a laboratory-generated pure component NH4 NO3 aerosol The instrument combines standard vacuum and mass spectrometric technologies with recently developed aerosol sampling techniques A unique aerodynamic aerosol inlet (developed at the University of Minnesota) focuses particles into a narrow beam and efficiently transports them into vacuum where aerodynamic particle size is determined via a particle time-of-flight (TOF) measurement Time-resolved particle mass detection is performed mass spectrometrically following particle flash
TL;DR: In this article, the authors discuss the role of chemical composition and particle size in cloud condensation nucleation processes, and the role that the chemical composition plays in the process of cloud droplet and ice nucleation.
Abstract: ARTICLE I NFO Atmospheric aerosol particles serve as condensation nuclei for the formation of both, cloud droplets and atmospheric ice particles. As a result, they exert a substantial influence on the microphysical properties of water and ice clouds, which in turn affect the processes that lead to the formation of rain, snow, hail, and other forms of precipitation. In recent years, considerable progress has been made in understanding the chemical composition of aerosols, their microphysical properties, and the factors that enable them to act as cloud condensation nuclei (CCN) and ice nuclei (IN). The first part of this review article will focus on the nature and sources of CCN and IN. We discuss the fundamentals of the cloud droplet and ice nucleation processes, and the role that the chemical composition and particle size play in this process. We show that, in many instances, the influence of chemical composition can be represented by a simple parameterization, which leaves particle size as the main variable controlling CCN efficiency. Aerosol particles are produced either directly by anthropogenic and natural sources (dust, sea salt, soot, biological particles, etc.), or they are formed in the atmosphere by condensation of low-volatility compounds (e.g., sulfuric acid or oxidized organic compounds). We discuss the magnitude of these sources, and the CCN and IN characteristics of the particles they produce. In contrast to previous assessments, which focused on the aerosol mass, we are emphasizing the number of particles being produced, as this is the key variable in cloud microphysics. Large uncertainties still exist for many aerosol sources, e.g., the submicron part of the seaspray aerosol, the particles produced by the biosphere, and the secondary organic aerosol. We conclude with a discussion on what particle concentrations may have been in the pristine atmosphere, before the onset on anthropogenic pollution. Model calculations and observations in remote continental regions consistently suggest that CCN concentrations over the pristine continents were similar to those now prevailing over the remote oceans, suggesting that human activities have modified cloud microphysics more than what is reflected in conventional wisdom. The second part of this review will address the effects of changing CCN and IN abundances on precipitation processes, the water cycle, and climate.